Rational Utilization of Intramolecular Hydrogen Bonds to Achieve Blue TADF with EQEs of Nearly 30% and Single Emissive Layer All-TADF WOLED.

A series of highly efficient blue thermally activated delayed fluorescence (TADF) compounds, SON-Cz, SON-tBuCz, and SON-PhCz, were developed. Pyridinyl was introduced as the bridging unit between carbazole donors and sulfone acceptor. Intramolecular hydrogen bonds between the pyridine N atom and carbazole H atoms were detected in single crystals, which suppressed the twisting of carbazole rings and dramatically increased the molecular rigidity. At the same time, tert-butyl or phenyl were incorporated at the 3,6-sites of carbazole ring to tune electron donating ability or enlarge HOMO delocalization. All these hydrogen bonds featured TADF compounds exhibited much improved photoluminescence quantum yields (PLQYs) and excellent efficiencies in their doped blue organic light-emitting diodes. In particular, SON-tBuCz and SON-PhCz exhibited the maximum external quantum efficiencies (EQEs) of 29.59% and 28.22% with CIE coordinates of (0.17, 0.22) and (0.21, 0.36), respectively. The excellent performance benefits from the carbazole structure modification and the intramolecular hydrogen bonds, which bring more rigid structures and eliminate nonradiative transitions. Furthermore, a single emissive layer all-TADF white OLED was fabricated using SON-tBuCz as the blue emitter and 4CzTPN-Ph as the orange emitter to give an EQE of 23.51% with a high CRI of 71, which is among the top efficiencies ever reported for all-TADF WOLEDs so far.